Devin O'Neill

Project description

DESCRIPTION PROJECT “Photography inspired activation of natural gas”

Formation of methyl halide by reaction with a halogen (bromine or chlorine) has been demonstrated to be a feasible very low energy pathway for CH4 activation. Subsequently the methyl halide can be coupled or hydrolyzed into alkanes, olefins or aromatics through catalysis over zeolites. Despite the significantly lower cost anticipated as compared to methane gasification and syngas chemistry, a major problem is the need for a halogen (Br2 or Cl2) with associated hazards and storage issues. This project investigates an alternative, solid metal halide based route, that precludes the dominant presence of Br2 or Cl2. In particular, we utilize the fact that single valent AgBr or CuBr compositions are excellent photocatalysts and halogen carriers. The HBr resulting from the reaction and processing of CH3Br to C-C coupling products over acidic catalysts, should be used to regenerate the initial solid catalyst (M+HBrMBr + H2, or M+HCl MCl+ H2) and close the catalytic cycle. We will determine the optimal catalyst morphology and process conditions making use among others of DFT calculations and sophisticated Raman and Infrared spectroscopic analyses, with emphasis on determining the catalytic feasibility of the halide conversion process by reaction with methane, as well as on the regeneration of the reduced catalyst by reaction with HBr (or HCl).

The main goals of the project are:

  • Determine the kinetics of light induced conversion of methane over metal halides by DFT (cooperation with Leigh university) and in situ vibrational spectroscopies
  • Determine the kinetics of the reaction of HBr or HCl with metal nanoparticles to the halide and H2
  • Optimize the catalyst composition and morphology, as well as process conditions